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Design of functionalized adsorbents for simultaneous removal of fluoride and arsenite from waters

同时去除水中氟化物和亚砷酸盐的功能化吸附剂的设计

基本信息

批准号：
16F16082
负责人：
笹木圭子
金额：
$ 1.41万
依托单位：
Kyushu University
依托单位国家：
日本
项目类别：
Grant-in-Aid for JSPS Fellows
财政年份：
2016
资助国家：
日本
起止时间：
2016-10-07 至 2019-03-31
项目状态：
已结题

项目摘要

It was aimed to synthesize a modulator (benzoic acid (BA))-driven zirconium-fumaric acid (Zr-fum) metal-organic frameworks (MOF) and investigated in detail the adsorption mechanism of arsenic oxyanions (AsO43- and AsO33-) and their stability before and after the adsorption from water. The mechanism of AsO43- and AsO33- interaction on Zr-MOF was ligand-exchange and found to be the maximum uptake performance of AsO43- (1.159 mmol/g) and AsO33- (1.121 mmol/g) was obtained by the Langmuir adsorption isotherm. Likewise, it is also synthesized La-based MOFs with the linkers of benzoic acid (BA), 1,4-benzene dicarboxylic acid (BDC) and 1,3,5-benzenetricarboxylic acid (BTC). Interestingly, the ligand of BA approached La metal to form lanthanum methanoate (La(HCOO)3 instead of La-BA MOF through acid catalyst amide-hydrolysis mechanism, where, La-BDC and La-BTC as MOFs, confirmed by PXRD patterns. This is the first report to investigate the AsO43- adsorption and their dissolution behavior over La-BA, La-BDC and La-BTC in detail using the different spectroscopic methods. The maximum adsorption capacities of AsO43- obtained from the Langmuir isotherm model were found to be 2.623 mmol/g, 3.891 mmol/g and 0.280 mmol/g for La-BA, La-BDC and La-BTC, respectively. The value for La-BDC was recorded as one of the much superior, next to UiO-66, to the previously reported adsorbents for AsO43- till date. In addition, the zirconia nanoparticles (ZrO2) embedded graphene oxide dendrimer was prepared and utilized for removal of toxic AsO33- removal from water.

合成了一种苯甲酸（BA）调控的富马酸锆（Zr-fum）金属有机骨架（MOF），并研究了其对水中砷氧阴离子（AsO 43-和AsO 33-）的吸附机理及其吸附前后的稳定性。结果表明，AsO 43-和AsO 33-在Zr-MOF上的吸附机理为配体交换，在Langmuir吸附等温线上，AsO 43-和AsO 33-的吸附量分别为1.159 mmol/g和1.121 mmol/g。同样，还合成了以苯甲酸（BA）、1，4-苯二甲酸（BDC）和1，3，5-苯三甲酸（BTC）为连接基的镧基MOFs。有趣的是，BA配体通过酸催化酰胺水解机理与La金属形成La（HCOO）3取代La-BA MOF，其中La-BDC和La-BTC为MOF，PXRD图谱证实了这一点。这是第一个报告，详细研究了AsO 43-吸附和溶解行为的La-BA，La-BDC和La-BTC使用不同的光谱方法。采用Langmuir等温吸附模型计算得到La-BA、La-BDC和La-BTC对AsO_（43-）的最大吸附容量分别为2.623 mmol/g、3.891 mmol/g和0.280 mmol/g。La-BDC的值被记录为仅次于UiO-66的上级吸附剂之一，优于先前报道的AsO 43吸附剂-迄今为止。此外，氧化锆纳米粒子（ZrO 2）嵌入氧化石墨烯树枝状大分子的制备和用于去除有毒AsO 33-去除从水中。